PNNL

Abstract

Accurate actinide measurements are critical within the field of nuclear science. Traditional methods for actinide quantification require time-consuming sample processing prior to analysis. There is a need for rapid analytical techniques that still maintain a high degree of accuracy. In this work, actinide reactivity was assessed for multiple oxygen-containing reaction gases using quadrupole inductively coupled plasma tandem mass spectrometry (Q-ICP-MS/MS) to evaluate actinide analysis in complex sample matrices without analyte-matrix separation. A novel method was developed to measure 241Am/241Pu in complex sample matrices using O2/He reaction gas with no matrix removal or analyte pre-concentration. This inline method reduces matrix-derived polyatomic interferences that complicate traditional ICP-MS analyses by mass-shifting to 241Am16O+ and 241Pu16O2+, allowing Am and Pu to be mass separated for simultaneous analysis. While mass shifting is efficient, a small portion of Am+ (1000 µg·g-1). Method detection limits of 15.9 fg·g-1 and 9.6 fg·g-1 were determined for 241Am and 241Pu, respectively, and 241Am/241Pu ratios were measured with accuracies within